Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 26
·20610-20619
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IF 9.5
Yutong Xia,Gege Wang,Jing Wu,Xiaowei Chi,Yu Liu
Aqueous zinc metal batteries (AZMBs) have garnered significant attention owing to the inherent safety of aqueous electrolytes and the zinc anode's high theoretical specific capacity (820 mA h g−1). However, interfacial instability arising from rampant zinc dendrite growth and parasitic side reactions at the electrolyte/anode interface critically hinders practical implementation. Herein, we report an in situ solid electrolyte interphase (SEI) engineering strategy via frustrated Lewis pair (FLP)-mediated polymerization of 2-acrylamido-2-methylpropane sulfonic acid (AMPS), where FLP catalysis is achieved through synergistic interactions between metallic zinc and Zn2+ cations at the electrolyte/anode interface. In contrast to conventional electrolyte additives that rely on physical adsorption or chemical passivation, the polymerized AMPS (PAMPS) establishes a dual-functional interface: (i) rapid Zn2+ ion transport channels through sulfonic acid groups, and (ii) robust chemical bonding with zinc via acrylamide moieties. This unique architecture enables simultaneous regulation of Zn2+ flux homogeneity and interfacial stabilization. Accordingly, Zn‖Zn symmetric cells with the AMPS-containing electrolyte show stable cycling for 6500 h at 1 mA cm−2. Notably, under extreme conditions (10 mA cm−2, 10 mA h cm−2), the PAMPS-enabled anode achieves a coulombic efficiency of 99.7% and an unprecedented cumulative areal capacity of 12 A h cm−2—a fourfold improvement over state-of-the-art benchmarks. Additionally, the MnO2‖Zn full cells with the AMPS-containing electrolyte exhibit a high specific capacity of 300 mA h g−1 at 500 mA g−1 and long cycling stability of 10 000 cycles at 1.58 A g−1. This work offers a facile, economical and effective approach for designing a high-performance aqueous zinc metal battery for practical applications.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2017
·Vol. 19
·期 28
·18232-18242
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IF 4.123
Samrat Devaramani,Mahgoub Ibrahim Shinger,Xiaofang Ma,Meng Yao,Shouting Zhang,Dongdong Qin,Xiaoquan Lu
J- and H-aggregates of zinc tetraphenylporphyrin (ZnTPP) on carbon nanotube films (CNTFs) were prepared using the mixed solvent method. This resulted in completely different structures, such as the four-leaf clover and flower, on the CNTF, which were observed by recording SEM images. Characteristic changes in the electronic spectra of the ZnTPP monomer appeared when it underwent J- and H-aggregation. The measured photocurrent significantly varied for the same molecule when it was aggregated in two different ways on ITO and ITO/CNTF. The electron recombination resistance of the two aggregates, which was investigated using electrochemical impedance spectroscopy, was also different. The photocatalytic efficiency of the J- and H-aggregates was examined by performing methylene blue dye decoloration studies. In addition, a scanning electrochemical microscope was used to investigate the photoinduced charge transfer kinetics of the J- and H-aggregates at the electrode/electrolyte interface as a fresh attempt. The heterogeneous charge transfer constants for the J- and H-aggregates in the presence of light at varied intensities were calculated. Thereby, striking differences in the photophysical, photocatalytic, and photoelectrochemical properties of the J- and H-aggregates were visualized throughout our studies.
研究领域:
材料科学
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光化学
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纳米技术
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电化学
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可再生能源
·
催化
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Hui Luo,Yunshu Yang,Liwen Lu,Guangxu Li,Xinhua Wang,Xiantun Huang,Xiaoma Tao,Cunke Huang,Zhiqiang Lan,Wenzheng Zhou,Jin Guo,Haizhen Liu
Li–Mg–B–H composite (2LiBH 4 + MgH 2 ) possesses a very high hydrogen storage capacity of 11.4 wt%. However, it still suffers from high operating temperature, slow kinetics, and poor reversibility. In this work, the two-dimensional Ti 3 CN MXene was first synthesized and then introduced into the Li–Mg–B–H composite. The addition of 5 wt% Ti 3 CN reduces the onset dehydrogenation temperature of the 2LiBH 4 + MgH 2 composite by about 50 °C and shortens the induction period of the LiBH 4 decomposition at 400 °C from >90 min to <10 min. The reversible capacity maintains at 8.3 wt% after 20 cycles, with a capacity retention ratio of 93%. Microstructure studies show that Ti 3 CN will partially transform to a highly-dispersed nano-TiB 2 with particle size around 5 nm. Such nano-TiB 2 could serve as an active catalyst to significantly improve the kinetics and reversibility of the Li–Mg–B–H composite. This work offers a strategy to enhancing the hydrogen storage performance of the advanced metal borohydride-based composites by addition of the MXene material and provides some new insights in understanding the role of MXene in tailoring the hydrogen storage properties of the Li–Mg–B–H composite.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Wei Yang,Yingqing Zhan,Qingying Feng,Ao Sun,Hongyu Dong
The rapid development of electronics puts forward higher requirements on the low dielectric materials . Especially, the polymer-based dielectric film with low dielectric constant , high thermal conductivity , and heat-resistance is essential to the flexible electronics. However, the balance of these intended performance is still a big challenge. In this work, we reported the flexible poly (arylene ether nitrile) (PEN) fibrous composite film with low dielectric constant and high thermal conductivity by coaxial electrospinning hot-pressing technique. Interestingly, such bi-functional fibrous composite film was rationally designed by using hexagonal boron nitride (h-BN)/fluorinated PEN (PEN-F) as shell layer and polyvinylpyrrolidone (PVP) as the core layer of fibers, which could further form the porous, hollow, and balsam pear-shaped structure after the hot-pressing and dissolution process. Owing to introduction of the h-BN nanosheets , intrinsic fluorine groups of PEN-F, and hollow nanofiber structure, the dielectric constant and dielectric loss of fibrous composite film could be as low as 1.74 and 0.0092 at 1 kHz, respectively. Furthermore, the in-plane thermal conductivity of fibrous composite film could reach 0.811 W m −1 K −1 by incorporation of 7 wt% h-BN. In addition, the fibrous composite film exhibited high thermal stability (T 5 % = 498 °C and T g = 182 °C) and mechanical strength (Tensile strength = 39.2 MPa and tensile modulus = 250.9 MPa). Therefore, this work opens up an alternative method to prepare high-performance polymer composite film with low dielectric constant and high thermal conductivity, which suggests the broad application in the future flexible electronics.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2020
·Vol. 21
·期 15
·5347
·
IF 4.556
Xiao-Ran Jing,Huan Liu,Yao Nie,Yan Xu
Fe(II)/2-ketoglutarate-dependent dioxygenase (Fe(II)/2-KG DO)-mediated hydroxylation is a critical type of C–H bond functionalization for synthesizing hydroxy amino acids used as pharmaceutical raw materials and precursors. However, DO activity requires 2-ketoglutarate (2-KG), lack of which reduces the efficiency of Fe(II)/2-KG DO-mediated hydroxylation. Here, we conducted multi-enzymatic syntheses of hydroxy amino acids. Using (2s,3r,4s)-4-hydroxyisoleucine (4-HIL) as a model product, we coupled regio- and stereo-selective hydroxylation ofl-Ile by the dioxygenase IDO with 2-KG generation from readily availablel-Glu byl-glutamate oxidase (LGOX) and catalase (CAT). In the one-pot system, H2O2significantly inhibited IDO activity and elevated Fe2+concentrations of severely repressed LGOX. A sequential cascade reaction was preferable to a single-step process as CAT in the former system hydrolyzed H2O2. We obtained 465 mM 4-HIL at 93% yield in the two-step system. Moreover, this process facilitated C–H hydroxylation of several hydrophobic aliphatic amino acids to produce hydroxy amino acids, and C–H sulfoxidation of sulfur-containingl-amino acids to yieldl-amino acid sulfoxides. Thus, we constructed an efficient cascade reaction to produce 4-HIL by providing prerequisite 2-KG from cheap and plentifull-Glu and developed a strategy for creating enzymatic systems catalyzing 2-KG-dependent reactions in sustainable bioprocesses that synthesize other functional compounds.Keywords:Fe(II)/2-ketoglutarate-dependent dioxygenase;2-ketoglutarate generation;regio- and stereo-selective synthesis;hydroxy amino acids;sequential cascade reaction
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2018
·
IF 2.829
Xueting Lu,Yangyang Li,Wei Feng,Shuang Guan,Peipei Guo
In this report, the self-healable hydrogels containing hydroxypropyl guar gum (HPG), acrylamide (AM) and 3-acrylamidophenylboronic acid (AAPBA) were prepared through a facile strategy. The double bond in AAPBA could polymerize with AM to form copolymers. Moreover, the boronic acid groups of AAPBA can interact with cis-diol of HPG which make AAPBA act not only polymer but cross-linkers simultaneously connecting PAM and HPG chains. The mechanical strength of the hydrogels was systematically investigated as a function of AAPBA content, HPG content, AM content and pH. It was found the hydrogels exhibited higher stress, elongations and self-healing properties due to the synergistic interaction of H-bond and dynamic covalent phenylboronic (PBA)-diol ester bonds. Furthermore, the hydrogels showed yielding phenomenon depending on the content of AM and pH, which could play a vital influence on the crosslinking manners and density. The detailed discussions of the relationship between crosslinking manners and yielding phenomenon provide a better understanding on the appearance of yielding phenomenon and their correlation with hydrogel structure.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Haizhen Liu,Liwen Lu,Hui Luo,Jiayi Deng,Guangxu Li,Hua Ning,Yi Fan,Cunke Huang,Zhiqiang Lan,Wenzheng Zhou,Jin Guo,Xinhua Wang
The Li-Mg-B-H composite (2LiBH 4 + MgH 2 ) is acknowledged as a promising material for hydrogen storage due to its large hydrogen capacity (11.4 wt.%). However, the sluggish kinetics and poor reversibility make it difficult to be practically used. In this work, the hydrogen storage performances of 2LiBH 4 + MgH 2 have been significantly improved by a hybrid of bulk NbC and layered Nb 4 C 3 MXene (denoted as “Nb-C”). The 2LiBH 4 + MgH 2 + 6 wt.% Nb-C can release 8.5 wt.% H 2 within 30 min at 400°C and the dehydrogenated composite can absorb 9.3 wt.% H 2 within 30 min at 350°C and 7.5 MPa H 2 . The reversible dehydrogenation capacity maintains at 8.4 wt.% after 24 cycles, with a capacity retention ratio of 95.4%. By contrast, the undoped 2LiBH 4 + MgH 2 suffers from serious capacity degradation, with the capacity decreased dramatically to 3.5 wt.% after 3 cycles. Microstructural studies revealed that the doped composite has uniform particle and elemental distributions and possesses various multiphase interfaces of LiH/MgB 2 /NbC/Nb 4 C 3 , which is beneficial to hydrogen diffusion during the hydrogen uptake and release process. Theoretical studies by first principle calculation presented an extended bond length of the Mg-H and B-H bonds in the 2LiBH 4 + MgH 2 + NbC system, which may also explain the improved hydrogen storage properties of 2LiBH 4 + MgH 2 by addition of Nb-C. This work provides new insights into the role of transition metal carbides in regulating the Li-Mg-B-H hydrogen storage materials both experimentally and theoretically.
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POLYMER COMPOSITES
·
2024
·
IF 4.8
Xinyi Jing,Linggong Meng,Tong Liu,Xinming Ye,Shuai Yang,Zhichao He,Wensheng Wang,Jie Li,Yingchun Li
Achieving high thermal conductivity in composites with low filler content is a major challenge in current research. In this paper, polypropylene (PP) and polyamide 6 (PA6) were used as polymer matrix, and the hybrid thermal conductive filler, formed by hexagonal boron nitride (h-BN) and aminated carbon nanotubes (NH 2 -CNTs), was integrated into matrix for the fabrication of thermal conductive composites (PP/PA6/h-BN and PP/PA6/h-BN@CNTs) via two-step melt blending technology. The thermal conductive fillers were selectively distributed in a phase of the polymer matrix with a co-continuous structure, forming a thermal conductive path with a three-dimensional network structure. The results show that when the content of h-BN reaches 25 wt%, the thermal conductivity of the PP/PA6/h-BN and PP/PA6/h-BN@CNTs composites was 199% and 300% higher than that of PP/PA6, respectively. Through testing the volume resistivity of the composites, it was confirmed that PP/PA6/h-BN@CNTs composites maintain good electrical insulation. Both composites demonstrated remarkable thermal conductivity and outstanding electrical insulation. This research provides a facile way to prepare highly thermal conductivity polymer composites with excellent processing performances and electrical insulation. Highlights h-BN@CNTs hybrid fillers with sandwich structure were prepared. A two-step blending method was used to control the selective distribution of hybrid fillers in a phase of the polymer matrix with a co-continuous structure. The hybrid filler formed a thermal conductive path with a three-dimensional network structure in the collective. PP/PA6/h-BN@CNTs composites demonstrated remarkable thermal conductivity, outstanding electrical insulation and favorable processing performances.
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CRYSTENGCOMM
·
2015
·Vol. 17
·期 11
·2376-2388
·
IF 4.034
Xiang-Sheng Zhai,Wen-Gang Zhu,Wei Xu,Ya-Jing Huang,Yue-Qing Zheng
Four new 3D uranyl complexes, [(UO2)2(H2O)(ipa)2]·9H2O (1), [(UO2)2(H2O)(nip)2]·H2O·Et3NH (2), [(UO2)2(H2O)(aip)2]·Et3NH (3) and [(UO2)(hip)]2·17H2O (4) (H2ipa = isophthalic acid, H2nip = 5-nitroisophthalic acid, H2aip = 5-aminoisophthalic acid, H2hip = 5-hydroxyisophthalic acid, Et3N = triethylamine), were hydrothermally synthesized. Structural analyses reveal that compounds 1–4 consist of pentagonal bipyramidal uranyl monomers bridged via acid inkers to form a structural motif, [(UO2)2L2], serving as the foundation of the 3D framework. Two structural motifs adopt different arrangement modes to connect to two types of chains. For 1–3, uranium atoms and carboxyl groups being from two types of chains respectively are coordinated to build similar 3D frameworks, while for 4, one type of chain links to the 3D architecture by the bond of the uranium atoms and –OH of the 5-hydroxyisophthalic acid ligand. The different guest molecules and structure assemblies displayed by the four compounds are a function of the variation of substituent groups of 5-X-1,3-benzenedicarboxylic acid (X = –H, –NO2, –NH2, –OH). Furthermore, the photocatalytic properties of 2 and 4 for degradation of rhodamine-B (RhB) upon xenon lamp irradiation have been examined. Elemental analysis, infrared spectroscopy, DRS and luminescence properties were also discussed.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 28
·6963-6972
·
IF 5.16
Yanji Zhu,Huaiyuan Wang,Kai Jin,Jinlong Gong
A graphene-wrapped polyaniline nanoparticles film embedded in carbon cloth (CC/PANI/G) was fabricated and used as a 3D anodic electrocatalyst for oxidation of toluene methyl C−H groups. The methyl C−H bonds can be oxidized effectively at the CC/PANI/G anode with 99.9 % toluene conversion at a low applied voltage of only 1.0 V, which implies low energy input. Importantly, 86.6 % of toluene methyl C−H groups were converted to benzoyl groups (C=O), and hydrogen was produced efficiently at the cathode. The electrocatalytic efficiency at the CC/PANI/G anode was higher at lower voltage (1.0 V) than at higher voltage (1.5 V), and more hydrogen was produced at the corresponding cathode. The synergistic effect between the dynamic redox chemistry of nanoPANI and the excellent conductivity and anticorrosive action of graphene determined the high electrocatalytic efficiency of the oxidation of toluene methyl C−H groups at the CC/PANI/G anode. Owing to the chemical bonding between graphene and PANI, the anticorrosive CC/PANI/G anodic electrocatalyst was durable and effective for oxidation of toluene methyl C−H groups in acidic environment. This approach provides advanced electrode materials for transforming stable chemical bonds (C−H) into useful functional groups (C=O), which will be beneficial for the synthesis of organic intermediates with coupled hydrogen production. Graphical It's a wrap : A graphene-wrapped polyaniline nanoparticles film embedded in carbon cloth was fabricated and used as an anodic electrocatalyst for oxidation of toluene methyl C−H groups (see figure). A toluene conversion of 99.9 % at a low applied voltage of only 1.0 V with 86.6 % conversion of toluene methyl C−H groups to benzoyl groups is coupled with efficient hydrogen production at the cathode.
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Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Jianwei Gao,Xiaoqing Si,Hanyue Ding,Xiaoyang Wang,Mushi Zheng,Chun Li,Junlei Qi,Jian Cao
Glass/Glass-ceramic sealing is always accompanied by issues of high porosity and brittle joints. To migrate these problems, an Ag foam was innovatively induced as an interlayer in the process of glass sealing the yttria-stabilized zirconia (YSZ) ceramic to Mn–Co spinel-coated Crofer 22 H stainless steel. Interlayer-added joints showed a significant reduction in porosity, and the shear strength was improved to 52.3 MPa, with an enhancement of 37.8 %. The influence of interlayer on the microstructure of the joint has been investigated and the formation process of the joint is illustrated. The Ag interlayer expels gases from the sealant material through expansion at high temperatures and promotes finer nucleation grains of crystallites integrating with the interlayer, reducing the porosity and alleviating the brittleness as well.
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CEMENT & CONCRETE COMPOSITES
·
2022
·
IF 9.93
Xing Ming,Qing Liu,Miaomiao Wang,Yongqing Cai,Binmeng Chen,Zongjin Li
Chloride-induced corrosion in reinforced concrete is a primary durability issue that causes large economic loss every year. To improve the intrinsic chloride binding capacity and realize a favorable corrosion protection of cement-based materials are thus crucial to prolong the service life of concrete structures. Here, alumina nano particles (ANPs) were incorporated to improve the chloride binding capacity of cement pastes in chloride solutions and the anti-corrosion performance of mortars under accelerated corrosion process. The ANPs facilitated the formation of alumino-ferrite-mono (AFm)-type phases, thereby improved the content of chemically bound chlorides. Solution calcium (Ca) ions benefited the chloride captured by calcium-(alumino-)silicate-hydrates (C-(A-)S-H) in the assistance of ANPs, especially at high initial chloride concentrations , and further evoked a pH-related chloride binding response. Moreover, the enhanced corrosion resistance was finally realized by incorporating appropriate amount of ANPs because of the filling and chemical effects induced low permeability of mortars. In general, the ANPs possess dual functions in the aspects of chloride binding and corrosion inhibition . These findings are expected to advance the design of high-durable cement-based materials serviced in the marine environment.
研究领域:
建筑材料
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土木工程材料
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腐蚀科学
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纳米材料应用
·
混凝土耐久性
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